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Session A24 - CMR I: Phase Separation I.
FOCUS session, Monday morning, March 12
Room 607, Washington State Convention Center

[A24.001] XAFS determination of local environment about Sr and La in CMR material, La_1-xSr_xMnO_3

Tomohiro Shibata, Bruce Bunker (Department of Physics, University of Notre Dame, Notre Dame IN 46556), Peter Schiffer (Department of Physics, Pennsylvania State University, University Park, PA 16802), John Mitchell (Materials Science Division, Argonne National Laboratory, Argonne IL 60439)

Sr doped lanthanum manganites La_1-xSr_xMnO_3 show colossal magnetoresistance effects that strongly depend on alloy composition. Many recent studies show the existence of charge, orbital, and spin ordering, and a number of anomalies have been observed in transport or magnetic properties. These properties have been generally been explained assuming that the sample composition is homogeneous through the entire sample. However, there is always the possibility for the non-random distribution of La and Sr atoms among the allowed sites with possible tendencies towards ordering or phase separation of the La and Sr atoms. Here we report XAFS studies of Sr K-edge and La K-edge to determine the local coordination of Sr around Sr and La atoms as a function of alloy composition. Our results do indeed indicate non-random site occupation for the Sr and La ions, and also show interesting anomalies in local lattice distortion as a function of alloy composition.

[A24.002] The metal-insulator transition in CMR manganites: a strange kind of percolation

Simon J. L. Billinge (Michigan State University)

The nature of the metal-insulator (MI) transition in colossal magnetoresistant manganites is still the subject of lively debate. Of note recently is the observation that both the ferromagnetic metallic and the paramagnetic insulating states below and above the MI transition, resepectively, are quite inhomogeneous. In this picture, the sample microscopically phase separates into metallic and insulating domains. The metal-insulator transition can then be understood in the framework of a percolation transition. Because of the strong coupling of the electronic system to the lattice through the Jahn-Teller distortion, this metal-insulator transition can be quantitatively studied using local structural probes such as the atomic pair distribution function (PDF) method. We discuss the nature of the MI transistor transition and show that it is not a conventional percolation transition and important physics beyond this simple percolation picture are necessary to explain the observations.

[A24.003] Recent Developments in the Phase Separation Theory of Manganites

Elbio Dagotto, Adriana Moreo, Matthias Mayr, Jan Burgy, Adrian Feiguin (National High Magnetic Field Lab and Department of Physics, Florida State University, Tallahassee, FL 32306, USA)

The present status of the mixed-phase scenario for manganites will be discussed(E. Dagotto, T. Hotta, and A. Moreo, to appear in Physics Reports.). Results include (a) the low-temperature coexistence of large equal-density ferromagnetic and antiferromagnetic clusters, and concomitant percolative process, when disorder influences on first-order transitions of the non-disordered limit(A. Moreo et al.), Phys. Rev. Lett. 84, 5568 (2000). , (b) calculations of resistivity vs temperature using a random-resistor network(M. Mayr et al.), Phys. Rev. Lett. 85, issue 26, Dec.2000. in agreement with experiments, (c) indications of a novel quantum critical behavior in the percolative regime (J. Burgy et al.), in preparation., and (d) the possibility of a new temperature scale T where clusters start forming above the Curie temperature.

[A24.004] Charge Ordering and Its Fluctuation in Manganites

S-W. Cheong (Department of Physics amp; Astronomy, Rutgers University and Bell Laboratories, Lucent Technologies), K. H. Kim, M. Uehara, B. G. Kim, V. Podzorov, M. Gershenson (Department of Physics amp; Astronomy, Rutgers University), C. H. Chen (Bell Laboratories, Lucent Technologies)

In doped Mott insulators, charge carriers tend to self-organize in such a way as to form stripe patterns at low temperatures. In the case of doped manganites, orbital degrees of freedom associated with Mn^3+ can be involved in the striped ordering. This striped charge/orbital ordering at low temperatures in manganites is associated with various length scales. Particularly, recent results indicate the presence of very-short-range or dynamic correlation of charge/orbital ordering at high temperatures, far above any phase transition temperatures. This significant fluctuation is directly associated with the origin of the colossal magnetoresistance effect.

[A24.005] Towards a test of the "bistripe" and Wigner Crystal models of charge ordering: approaches to crystal growth of LCMO (x=2/3)

John Mitchell (Materials Science Divsion, Argonne National Laboratory), Hong Zheng (Materials Science Divsions, Argonne National Laboratory), Dean Miller, Dimitri Argyriou (Materials Science Division, Argonne National Laboratory)

The mode of charge ordering of Mn(III) and Mn(IV) ions in the heavily doped (x>0.5) LCMO system remains in controversy. Lattice images of samples from this region of the phase diagram indicate a fascinating "bistripe" arrangement in which Mn(III) pairs interleave with Mn(IV) regions. The spacing of these bistripes is determined by the Ca concentration. In contrast, neutron diffraction on bulk samples indicates a more homogeneous distribution of the dilute Mn(III) ions, whose arrangement into a Wigner lattice minimizes the Coulomb energy of the ensemble. Refinement of the powder neutron data relied on comparing intensity of weak superlattice reflections to model predictions. To reconcile these disparate models, we have undertaken growth of single crystals of the x=2/3 composition in the solid solution. In this talk we discuss the issues facing the successful crystal growth of this system including process parameters that impact the crystal growth process.

[A24.006] Raman Scattering and Ellipsometric Studies of the Charge-Ordered Phase of (Bi,Ca)MnO3*

S. L. Cooper (Department of Physics and Frederick Seitz Materials Research Laboratory, University of Illinois, Urbana-Champaign)

We have studied the dramatic effects of charge ordering on the charge-, spin-, and lattice-dynamics of the (Bi,Ca)MnO3 system using spectroscopic ellipsometry and Raman scattering. By probing the dielectric anisotropy at different temperatures and energies, spectroscopic ellipsometry has allowed us to study how charge-ordering influences the charge- and orbital degrees of freedom on various length scales. Among other effects, we observe evidence for significant charge-stripe fluctuations above the charge-ordering transition, and for different temperature dependencies associated with charge- and orbital-ordering. The temperature evolution of the dielectric anisotropy also exhibits interesting similarities with the development of the phonon spectrum probed by Raman scattering, which reveals evidence for anisotropic lattice dynamics and the activation of forbidden phonon modes below the charge-ordering transition. Additionally, we observe in the antiferromagnetic charge-ordered phase the development of a quasielastic light scattering response having a distinctive T1g symmetry. This unusual scattering symmetry transforms like the spin-chirality operator (S1*S2xS3), and thus this quasielastic response betrays the presence of strong magnetic or chiral fluctuations at finite temperatures in the antiferromagnetic charge-ordered phase. As will be discussed, among the possible sources of this anomalous response are (i) fluctuations of the core spins associated with a canted antiferromagnetic or spin-chiral phase, and (ii) fluctuations associated with closed-loop charge currents, arising from the strong constraints placed on conduction by the complex spin-texture of the Neel state and the double-exchange hopping mechanism.

*This work was supported in part by the Department of Energy under DEFG02-96ER4539, and was performed in conjunction with S. Yoon, M. Ruebhausen, K. H. Kim, and S-W. Cheong.

[A24.007] Phase segregation in manganite perovskites: FM clusters at the crossover between two AFM states

Chris Ling (Argonne National Laboratory), John Neumeier (Florida Atlantic University), Dimitri Argyriou (Argonne National Laboratory)

The CMR perovskite La_1-xCa_xMnO_3 has been relatively neglected in high-x region. Magnetic susceptibility measurements suggest the presence of small FM clusters in the crossover region between the Type-C and Type-G AFM states. A phase transition intimately associated with the C-AFM (but not G-AFM) state has allowed us to determine with which AFM phase the FM clusters are associated, via a combination of synchrotron XRD and neutron powder diffraction. The high-symmetry phase was found to contain a FM component in addition to G-AFM, but the low-symmetry phase was found to contain no FM component in addition to C-AFM. Furthermore, there is evidence that below T_N(G), the low-symmetry phase associated with C-AFM is slowly colonized by G-AFM, similar to our recent observations of the analogous pseudo-2D system La_2-2xSr_1+2xMn_2O_7.

This work was supported by the Office of Science, US DOE, under contract W-31-109-ENG-38 (CL, DA) and by the NSF under contract DMR 9982834 (JN).

[A24.008] Mesoscopic, Non-equilibrium Fluctuations of Inhomogeneous Electronic States in Manganites

V. Podzorov (Serin Physics Laboratory, Rutgers University, Piscataway, NJ 08854), C. H. Chen (Bell Laboratories, Lucent Technologies, Murray Hill, NJ 07974), M. E. Gershenson, S-W. Cheong (Serin Physics Laboratory, Rutgers University, Piscataway, NJ 08854)

By using the dark-field real-space imaging technique of transmission electron microscopy (TEM), we have observed slow 200 Å-scale fluctuations of charge-ordered (CO) phase in mixed-valent manganites under a strong electron beam irradiation. These unusual fluctuations of the CO phase are related to the switching-type fluctuations of electrical esistivity, which were found to be as large as several percents. Systematic analysis indicates that this slow dynamics with a time scale of the order of seconds originates from non-equilibrium processes, and a meta-stable, charge-"disordered" insulating phase, plays an essential role in the observed fluctuations.

[A24.009] Thermodynamics and Kinetics of Mesoscopic Phase Fluctuations in a Bulk CMR Crystal

Frank Hess, Robert Merithew, Mike Weissman (University of Illinois at Urbana-Champaign), Y. Tokura, Y. Tomioka (Joint Research Center for Atom Technology)

We observe discrete two-state conductance fluctuations at the CMR transition in a bulk La_0.66Ca_0.33MnO_3 single crystal (R.D Merithew et. al. PRL \textbf84, 3442 (2000)). The magnetic moment and entropy differences between the two resistance states are determined from the temperature and field dependences of the switchers' duty cycles. The resulting entropy to magnetic moment ratios are similar to results obtained from conventional heat capacity and magnetization measurements. Analysis of the switchers' transition rates show the barrier state has moment and entropy intermediate between the two stable end states, as would be natural for a domain switching between a ferromagnetic, low entropy phase and a paramagnetic, high entropy phase. Switchers which persist after the sample has undergone temperature cycles into the insulating phase and back indicate the detailed structure of the mixed phase is partially determined by quenched disorder. This work was supported by NSF DMR 99-81869.

[A24.010] Optical investigation of La_1-xCa_xMnO_3 (x=0.48, 0.5, and 0.52)

K. H. Kim, T.W. Noh (School of Physics, Seoul National University, Seoul 151-742, Korea), S.-W. Cheong (Dept. of Physics and Astronomy, Rutgers University, Piscataway, NJ 08854 and Bell Laboratories, Lucent Technologies, Murray Hill, NJ 07974)

We investigated temperature (T)-dependent optical conductivity spectra \sigma (ømega ) of La_1-xCa_xMnO_3 (% x=0.48, 0.5, and 0.52). \sigma (ømega ) of x=0.48 and 0.50 samples exhibit two absorption bands in a mid-infrared region at 10 K, showing clearly a coexistence of both ferromagnetic metallic and charge orderded (CO) insulating domains in these compounds. Doping dependence of \sigma (ømega ) at 10 K reveals that charge gap due to the CE type CO, stabilized in La_1-xCa_xMnO_3 near x=0.5, is \sim 0.5 eV, which is quite higher than a previously reported value of \sim 0.1 eV. On the other hand, above T_CO, all the compounds have a broad mid-infrared absorption band centered around 1.0 eV, accompanied by a pseudogap feature at a lower frequency region. The pseudogap behavior of x=0.5 becomes more evident than those of x=0.48 and 0.52, suggesting that a short-range CO correlation persisting at a high T region can be closely related to the observed pseudogap behavior.

Part A of program listing